867 research outputs found

    One pot ‘click’ reactions: tandem enantioselective biocatalytic epoxide ring opening and [3+2] azide alkyne cycloaddition

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    Halohydrin dehalogenase (HheC) can perform enantioselective azidolysis of aromatic epoxides to 1,2-azido alcohols which are subsequently ligated to alkynes producing chiral hydroxy triazoles in a one-pot procedure with excellent enantiomeric excess.

    Exploring molecular motors

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    The introduction of mechanical functions and controlled motion based on molecular motors and machines offers tremendous opportunities towards the design of dynamic molecular systems and responsive materials. In this brief perspective the focus is on the exploration of rotary molecular motors discussing basic principles and showing illustrative applications in functional materials. Furthermore, major challenges to bring dynamic properties to more complex molecular systems, ranging from transmission, amplification and synchronization to biocompatibility and autonomous behavior, are discussed

    Spin Relaxation in Graphene with self-assembled Cobalt Porphyrin Molecules

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    In graphene spintronics, interaction of localized magnetic moments with the electron spins paves a new way to explore the underlying spin relaxation mechanism. A self-assembled layer of organic cobalt-porphyrin (CoPP) molecules on graphene provides a desired platform for such studies via the magnetic moments of porphyrin-bound cobalt atoms. In this work a study of spin transport properties of graphene spin-valve devices functionalized with such CoPP molecules as a function of temperature via non-local spin-valve and Hanle spin precession measurements is reported. For the functionalized (molecular) devices, we observe a slight decrease in the spin relaxation time ({\tau}s), which could be an indication of enhanced spin-flip scattering of the electron spins in graphene in the presence of the molecular magnetic moments. The effect of the molecular layer is masked for low quality samples (low mobility), possibly due to dominance of Elliot-Yafet (EY) type spin relaxation mechanisms

    Enlightening dynamic functions in molecular systems by intrinsically chiral light-driven molecular motors

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    Chirality is a fundamental property which plays a major role in chemistry, physics, biological systems and materials science. Chiroptical artificial molecular motors (AMMs) are a class of molecules which can convert light energy input into mechanical work, and they hold great potential in the transformation from simple molecules to dynamic systems and responsive materials. Taking distinct advantages of the intrinsic chirality in these structures and the unique opportunity to modulate the chirality on demand, chiral AMMs have been designed for the development of light-responsive dynamic processes including switchable asymmetric catalysis, chiral self-assembly, stereoselective recognition, transmission of chirality, control of spin selectivity and biosystems as well as integration of unidirectional motion with specific mechanical functions. This review focuses on the recently developed strategies for chirality-led applications by the class of intrinsically chiral AMMs. Finally, some limitations in current design and challenges associated with recent systems are discussed and perspectives towards promising candidates for responsive and smart molecular systems and future applications are presented.</p

    Light-driven Rotary Molecular Motors for Out-of-Equilibrium Systems

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    This chapter discusses whether rotary molecular motors are able to operate away from thermal equilibrium and whether this work on the molecular scale can be amplified across length scales and light-driven rotary motors. The chapter analyzes examples from literature demonstrating the ability of molecular motors to perform work, starting with examples in which a net output is generated by single molecules, followed by larger (supramolecular) systems. The molecular motors are overcrowded alkene switches, and the initial establishment of a photostationary state can be recognized as the photochemical equilibrium described for photoswitches. Surface immobilization is the possibilities to overcome Brownian motion and give opportunity to turn the relative rotation of one motor half with respect to the other into an absolute rotation of the motor with respect to the surface. Self-assembly opens up the possibility to work with very complex systems and enhance functions through cooperativity without the need of complicated synthesis of elaborate single molecules.</p

    Fast synthesis and redox switching of di- And tetra-substituted bisthioxanthylidene overcrowded alkenes

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    A rapid and efficient method for the synthesis of overcrowded alkenes using (trimethylsilyl)diazomethane provides a range of substituted bisthioxanthylidenes. We show large conformational redox switching from folded to orthogonal states, which tolerates many substitution patterns. The facile access to bisthioxanthylidene switches with the potential for further functionalization, in combination with the reliable redox chemistry, provides major opportunities for the design of electrochemically responsive systems

    Designing light-driven rotary molecular motors

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    The ability to induce and amplify motion at the molecular scale has seen tremendous progress ranging from simple molecular rotors to responsive materials. In the two decades since the discovery of light-driven rotary molecular motors, the development of these molecules has been extensive; moving from the realm of molecular chemistry to integration into dynamic molecular systems. They have been identified as actuators holding great potential to precisely control the dynamics of nanoscale devices, but integrating molecular motors effectively into evermore complex artificial molecular machinery is not trivial. Maximising efficiency without compromising function requires conscious and judicious selection of the structures used. In this perspective, we focus on the key aspects of motor design and discuss how to manipulate these properties without impeding motor integrity. Herein, we describe these principles in the context of molecular rotary motors featuring a central double bond axle and emphasise the strengths and weaknesses of each design, providing a comprehensive evaluation of all artificial light-driven rotary motor scaffolds currently present in the literature. Based on this discussion, we will explore the trajectory of research into the field of molecular motors in the coming years, including challenges to be addressed, potential applications, and future prospects.</p

    Designing light-driven rotary molecular motors

    Get PDF
    The ability to induce and amplify motion at the molecular scale has seen tremendous progress ranging from simple molecular rotors to responsive materials. In the two decades since the discovery of light-driven rotary molecular motors, the development of these molecules has been extensive; moving from the realm of molecular chemistry to integration into dynamic molecular systems. They have been identified as actuators holding great potential to precisely control the dynamics of nanoscale devices, but integrating molecular motors effectively into evermore complex artificial molecular machinery is not trivial. Maximising efficiency without compromising function requires conscious and judicious selection of the structures used. In this perspective, we focus on the key aspects of motor design and discuss how to manipulate these properties without impeding motor integrity. Herein, we describe these principles in the context of molecular rotary motors featuring a central double bond axle and emphasise the strengths and weaknesses of each design, providing a comprehensive evaluation of all artificial light-driven rotary motor scaffolds currently present in the literature. Based on this discussion, we will explore the trajectory of research into the field of molecular motors in the coming years, including challenges to be addressed, potential applications, and future prospects
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